Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0124910.1021/acs.energyfuels.5c01249
Erasto E. Kasala*, Jinjie Wang*, Asia Majid, Mbula Ngoy Nadege and Edwin E. Nyakilla,
{"title":"Review and Perspectives on Enhancing the Hydrogen (H2) Storage Capacity and Stability in Geological Formations via Nanoparticle-Assisted Surfactant/Polymer Formulations","authors":"Erasto E. Kasala*, Jinjie Wang*, Asia Majid, Mbula Ngoy Nadege and Edwin E. Nyakilla, ","doi":"10.1021/acs.energyfuels.5c0124910.1021/acs.energyfuels.5c01249","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01249https://doi.org/10.1021/acs.energyfuels.5c01249","url":null,"abstract":"<p >Despite numerous laboratory and simulation findings with great potential, nanoparticles (NPs), surfactants, and polymers used for enhancing hydrogen (H<sub>2</sub>) storage capacity and stability in geological formations face significant challenges. Their long-term stability is compromised in the harsh conditions of sediment heterogeneity, overly high pressure and temperature, pH changes, sediment interactions, and fluctuation in salinity, which impede large-scale implementation. Incorporating NPs into surfactants and polymers yields a nanofluid revealing increased viscosity, enhanced dispersion, improved wettability, enhanced surface interaction, H<sub>2</sub> uptake, H<sub>2</sub> solubility, increased retention, and long-term stability─ultimately leading to long-term H<sub>2</sub> storage efficiency, all attributable to the synergistic effects of their components. In this research, the performance efficiency of NP-assisted surfactant/polymer formulations and the factors that impair their effectiveness were highlighted. Numerous NP-assisted surfactant/polymer formulations’ adsorption/absorption mechanisms, such as size-dependent interactions, surface charge effects, aggregation behavior, interfacial tension (IFT) modulation, H<sub>2</sub> bonding, and hydrophobic interactions on the aqueous phase, were illustrated. The synergistic interaction of NP-assisted surfactant or polymer to the IFT reduction, improved rheological properties, flow stability, H<sub>2</sub> adsorption, dispersion efficiency, phase retention, enhanced storage capacity, and long-term stability were also presented. Nevertheless, the extent of the synergy observed depends on the specific type and property of NPs, surfactants, or polymers used. In addition, the review highlighted the existing challenges, research gaps, and proposed potential interventions. The research uniquely bridges the gap between molecular-level interactions and field-scale applications, offering a novel synthesis of experimental and simulation data to propose actionable solutions for overcoming current limitations in H<sub>2</sub> storage technology. By focusing on the underexplored synergy of nanoparticle-surfactant/polymer systems in geological H<sub>2</sub> storage, this work advances the understanding of how nanoscale modifications can optimize macroscale storage efficiency and stability.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10165–10199 10165–10199"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0047210.1021/acs.energyfuels.5c00472
Anton S. Perera, Yilin Wang, Sashen Ruhunage, Lily A. Robertson, T. Malsha Suduwella, Sean R. Parkin, Randy H. Ewoldt, Chad Risko* and Aman Preet Kaur*,
{"title":"Decoding the Effect of Anion Identity on the Solubility of N-(2-(2-Methoxyethoxy)ethyl)phenothiazine (MEEPT)","authors":"Anton S. Perera, Yilin Wang, Sashen Ruhunage, Lily A. Robertson, T. Malsha Suduwella, Sean R. Parkin, Randy H. Ewoldt, Chad Risko* and Aman Preet Kaur*, ","doi":"10.1021/acs.energyfuels.5c0047210.1021/acs.energyfuels.5c00472","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00472https://doi.org/10.1021/acs.energyfuels.5c00472","url":null,"abstract":"<p >Variations in the solubility of redox-active organic molecules (ROM) of interest for nonaqueous redox flow batteries (RFB), especially as the ROM state-of-charge changes during charge–discharge cycling, present significant molecular design challenges. The situation is further complicated as ROM solubility can be regulated by the choice of electrolyte salt and solvent that together with the ROM comprise the catholyte or anolyte (redox electrolyte) formulation, presenting materials design challenges. The ROM <i>N</i>-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT) is a viscous liquid at room temperature and is miscible in several organic solvents, including acetonitrile and propylene carbonate. The MEEPT radical cation (MEEPT<sup>+•</sup>) paired with tetrafluoroborate (BF<sub>4</sub><sup>–</sup>) in acetonitrile presents a 0.5 M solubility, a dramatic decrease when compared to the viscous liquid of neutral MEEPT. Here we present a joint experimental, regression modeling, and molecular dynamics (MD) simulations investigation to explore MEEPT–X (where X represents the counteranion) salt solubility variability as a function of concentration and counteranion chemistry in acetonitrile. We find a strong dependence of the salt solubility on the counteranion and relate these findings to explicit intermolecular interactions between MEEPT<sup>+•</sup> and the counteranion in the electrolyte solution.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10649–10658 10649–10658"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0144410.1021/acs.energyfuels.5c01444
Mark Romanczyk*, Jeffrey A. Cramer, Kristina M. Myers and Thomas N. Loegel,
{"title":"High-Resolution Mass Spectrometry Reveals Heteroatom-Based Compositional Trends Linked to Jet Fuel Instability","authors":"Mark Romanczyk*, Jeffrey A. Cramer, Kristina M. Myers and Thomas N. Loegel, ","doi":"10.1021/acs.energyfuels.5c0144410.1021/acs.energyfuels.5c01444","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01444https://doi.org/10.1021/acs.energyfuels.5c01444","url":null,"abstract":"<p >When exposed to high heat, the nitrogen- and oxygen-containing compounds (NCCs and OCCs, respectively) in fuels react to form oxidative deposits that may result in fuel failures. Due to the complexity of fuel, it is arduous to assign which class(es) of NCCs and OCCs exhibit the greatest propensities to form these adverse deposits. Hence, there is a burgeoning need to qualitatively characterize stable and thermally unstable jet fuels and compare their compositions. If links between compositions and fuel stability are realized, the harmful compounds can be identified and targeted for removal, consequently improving the fuel quality. The central aims of this work were to (1) qualitatively characterize ionized NCCs and OCCs derived from stable and unstable jet fuels, (2) compare and contrast the NCC and OCC compositions of stable and unstable fuels, (3) denote links between composition and thermally unstable fuels, and (4) utilize automated cluster optimization via serial variable down-selection and singular value decomposition to confirm manual assessments of data linkages. To complete the characterization, (+) and (−) electrospray ionization coupled to a high-resolution Orbitrap mass spectrometer was utilized. Upon measurement, the unstable fuels had greater abundances of OCCs with ≥2 oxygen atoms and ions with empirical formulas of C<sub><i>n</i></sub>H<sub>(2<i>n</i>-1)</sub>O<sub>2</sub>, C<sub><i>n</i></sub>H<sub>(2<i>n</i>-3)</sub>O<sub>2</sub>, and C<sub><i>n</i></sub>H<sub>(2<i>n</i>-5)</sub>O<sub>2</sub>. Furthermore, although stable fuels contained a balanced distribution of different classes of NCCs, unstable fuels had a relatively large abundance of ions with a specific empirical formula of C<sub><i>n</i></sub>H<sub>2<i>n</i>-6</sub>N. Additional qualitative information was reported, including Kendrick Mass Defect plots. Overall, NCC and OCC compositional differences were noted when stable and unstable fuels were compared, highlighting the proficiency of the Orbitrap at characterization. Although it remains uncertain if these differences are responsible for fuel failure, the emergence of links between fuel compositions and thermal instability may prove critical at identifying the class(es) that pose the most harm to fuel.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10331–10345 10331–10345"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211886","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0215110.1021/acs.energyfuels.5c02151
Jianchao Cai*, and , Steffen Berg*,
{"title":"Recent Advances in Flow Through Porous Media for Energy Exploitation","authors":"Jianchao Cai*, and , Steffen Berg*, ","doi":"10.1021/acs.energyfuels.5c0215110.1021/acs.energyfuels.5c02151","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c02151https://doi.org/10.1021/acs.energyfuels.5c02151","url":null,"abstract":"","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 20","pages":"9181–9184 9181–9184"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104884","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0099610.1021/acs.energyfuels.5c00996
Kunlin Ma, Dongliang Li*, Jingsheng Lu, Decai Lin and Deqing Liang,
{"title":"Analysis of Hydrate Formation Kinetics and Wall-Climbing Growth Regulation Using Biofriendly Promoters: Synergistic Effects of Erioglaucine Disodium Salt and Sugar Alcohol","authors":"Kunlin Ma, Dongliang Li*, Jingsheng Lu, Decai Lin and Deqing Liang, ","doi":"10.1021/acs.energyfuels.5c0099610.1021/acs.energyfuels.5c00996","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00996https://doi.org/10.1021/acs.energyfuels.5c00996","url":null,"abstract":"<p >The high toxicity, excessive foaming, and wall-climbing behavior of traditional promoters limit their large-scale use in hydrate-based gas storage and separation. Environmentally friendly and efficient hydrate management strategies are needed. We used a sapphire cell for comparative analysis of kinetic dynamics and wall-climbing morphology during hydrate formation under sugar alcohol (SA) and erioglaucine disodium salt (EDS). Microscopic analyses explored the mechanisms of EDS and SA on hydrate formation, with comparisons to amino acids. This is the first report on the synergistic effects of SA and EDS, both of which exhibit excellent biocompatibility and degradability, not only in significantly enhancing hydrate formation but also in regulating hydrate wall-climbing behavior. Three distinct modes of hydrate wall-climbing were observed at varying concentrations of EDS and SA. At a concentration of 4 ppm EDS + SA, hydrates exhibited an “antenna growth” mode, characterized by delayed promotion and a significantly prolonged induction time compared to the film formation time. In contrast, 200 ppm EDS + SA demonstrated a strong synergistic effect, drastically reducing both film formation and induction times. Microscopic characterizations revealed that while EDS + SA enhanced the selectivity of the hydrate for CO<sub>2</sub>, it did not alter the hydrate cage structure. Optical microscopy results further demonstrate that EDS + SA can inhibit the capillary growth of hydrates and alter their crystal morphology. These findings suggest a mechanism in which a hydrophobic skeletal network promotes hydrate formation and regulates wall-climbing behavior. The EDS + SA combination holds promise for large-scale hydrate applications, offering efficient promotion and wall-climbing control.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10374–10393 10374–10393"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211798","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0148810.1021/acs.energyfuels.5c01488
Babalola Aisosa Oni*, Ismail Akamu Adebayo, Victor Oyebamiji Ojo and Christopher Nkansah,
{"title":"Insight into Underground Hydrogen Storage in Aquifers: Current Status, Modeling, Economic Approaches and Future Outlook","authors":"Babalola Aisosa Oni*, Ismail Akamu Adebayo, Victor Oyebamiji Ojo and Christopher Nkansah, ","doi":"10.1021/acs.energyfuels.5c0148810.1021/acs.energyfuels.5c01488","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01488https://doi.org/10.1021/acs.energyfuels.5c01488","url":null,"abstract":"<p >Aquifers are considered one of the most eco-friendly forms of underground hydrogen storage due to their widespread availability, natural porosity, minimal requirement for structural modification, and reduced environmental disruption compared to other options, such as salt caverns or depleted reservoirs. However, the number of active aquifer-based hydrogen storage projects is limited, as most current storage efforts focus on depleted fields and salt caverns. Unlike salt caverns, which require extensive mining and energy-intensive leaching processes or depleted reservoirs that may pose risks of residual hydrocarbons contaminating stored hydrogen, aquifers typically involve fewer invasive preparatory measures. Additionally, their wide geographical distribution makes them accessible without significant infrastructure development, reducing the carbon footprint associated with site preparation and operation. With careful monitoring to mitigate risks, such as microbial hydrogen consumption, aquifers offer a sustainable and less intrusive alternative for large-scale hydrogen storage. This is crucial for scaling up hydrogen as a primary energy carrier in global decarbonization efforts. While aquifers show high potential, their use for hydrogen storage remains underdeveloped, requiring significant research and development investment. Hydrogen’s interaction with aquifer materials poses risks, necessitating rigorous site assessments and mitigation strategies. Despite existing challenges, economic assessments indicate that aquifer costs are unpredictable due to a lack of reservoir characterization. This review further discusses the geological properties, H<sub>2</sub> loss pathway and mitigation strategies, sealing technologies, potential storage sites, challenges and economic analysis of H<sub>2</sub> storage in aquifers.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10274–10303 10274–10303"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0090310.1021/acs.energyfuels.5c00903
Ashawari Dewri, Gaurisankar Phukan, Salma A. Khanam, Donguk Kim, Young-Bin Park and Kusum K. Bania*,
{"title":"Tin Oxide with Trace Metallic Rhodium (0) Impurity for Overall Water Splitting Reaction: Impact of Rh Loading and Twin Boundaries","authors":"Ashawari Dewri, Gaurisankar Phukan, Salma A. Khanam, Donguk Kim, Young-Bin Park and Kusum K. Bania*, ","doi":"10.1021/acs.energyfuels.5c0090310.1021/acs.energyfuels.5c00903","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00903https://doi.org/10.1021/acs.energyfuels.5c00903","url":null,"abstract":"<p >Tin oxide (SnO<sub>2</sub>) loaded with a variable concentrations of metallic rhodium (Rh) was explored for the overall splitting of water (H<sub>2</sub>O) in an alkaline medium. Three different catalysts, viz. Rh-SnO<sub>2</sub>-I, Rh-SnO<sub>2</sub>-II and Rh-SnO<sub>2</sub>-III, with different Rh-to-Sn ratios, were evaluated for simultaneous oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) processes in 1 M KOH. The catalyst Rh-SnO<sub>2</sub>-I, with low Rh loading, showed better OER activity with an onset potential of 1.45 V and an overpotential (<i>η</i>) of 240 mV, while the same for HER was found to be 470 mV. The Rh-SnO<sub>2</sub>-II catalyst, with Rh loading slightly higher than that of Rh-SnO<sub>2</sub>-I, showed OER activity with <i>η</i> = 250 mV and HER activity with <i>η</i> = 226 mV. The Rh-SnO<sub>2</sub>-III catalyst, with the highest Rh content and twin boundaries, was found to show superior HER activity with <i>η</i> of 222 mV at a current density (J) of 10 mAcm<sup>–2</sup>. The OER and HER activity in all cases were found to decrease at low pH. Tafel plot analysis and other comparative studies indicated that the loading of Rh into SnO<sub>2</sub> substantially altered the OER and HER activity. The lowest Tafel slope of 200 mVdec<sup>–1</sup> in OER was found in the case of Rh-SnO<sub>2</sub>-I. Rh-SnO<sub>2</sub>-III catalyst had the lowest Tafel slope value of 128 mVdec<sup>–1</sup> in HER. The current study implied that the introduction of Rh in SnO<sub>2</sub> can improve the HER activity and OER activity depending on the loading of Rh content. Density Functional Theory (DFT) calculations were used to understand the mechanism of overall water-splitting reactions. The study suggested that the water-splitting reaction would be more favorable if the hydrolysis process proceeded through the abstraction of hydrogen (H<sub>2</sub>) at the Rh center. The formation of the Sn–H bond during the second H<sub>2</sub> molecule liberation was detected to be the rate-determining step.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10594–10609 10594–10609"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-22DOI: 10.1021/acs.energyfuels.5c0086210.1021/acs.energyfuels.5c00862
Khawaja Hasnain Iltaf, Qinhong Hu*, Majie Fan, Prince Oware, Qiming Wang, Chen Zhao, Tao Zhang, Rizwan Sarwar Awan, Danish Khan and Ali Raza,
{"title":"Multiscale Pore Characterization of the New Albany Shale: Insights from Complementary Analytical Techniques","authors":"Khawaja Hasnain Iltaf, Qinhong Hu*, Majie Fan, Prince Oware, Qiming Wang, Chen Zhao, Tao Zhang, Rizwan Sarwar Awan, Danish Khan and Ali Raza, ","doi":"10.1021/acs.energyfuels.5c0086210.1021/acs.energyfuels.5c00862","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00862https://doi.org/10.1021/acs.energyfuels.5c00862","url":null,"abstract":"<p >The extraction of hydrocarbons from shale formations has become increasingly important, necessitating a deeper understanding of their morphological and structural characteristics, particularly pore types and pore structure parameters, which are essential for determining the storage and productive potential of shale oil reservoirs. This research addresses this need by investigating the distribution, formation, and mineralogical relationships of pores in the three lithofacies of the New Albany Shale (NAS) in the Illinois Basin. Utilizing scanning electron microscopy (SEM), nitrogen (N<sub>2</sub>) physisorption, small-angle X-ray scattering (SAXS), X-ray diffraction (XRD), polarizing microscopy, and TOC analyses, the study comprehensively analyzes the pore structure and morphology across these lithofacies. The Brunauer–Emmett–Teller (BET) specific surface area (SSA) ranges from 0.3 to 24.6 m<sup>2</sup>/g (average of 5.5 m<sup>2</sup>/g), with the total pore volume (TPV) ranging from 0.002 to 0.040 cm<sup>3</sup>/g (average 0.012 cm<sup>3</sup>/g). The results reveal that NAS exhibits a heterogeneous pore structure, characterized by various pore sizes and shapes, varying from ink-bottle-shaped in lithofacies NAS-1 and NAS-2 to predominantly wedge-shaped in lithofacies NAS-3. Inorganic pores, including mesopores and macropores, play a significant role in the pore system, and their presence is influenced by the specific lithofacies types within NAS. Organic matter (OM) pores exhibit limited development across all lithofacies, which could be attributed to the lower thermal maturity. In contrast, microfractures associated with organic matter and brittle minerals are comparatively well-developed. The NAS-2 lithofacies is particularly important for fluid migration due to its favorable pore structure parameters. A detailed understanding of the mechanisms of pore formation and their structural attributes across different minerals and lithofacies is crucial for advancing the exploration and development of shale oil and gas deposits.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10356–10373 10356–10373"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-21DOI: 10.1021/acs.energyfuels.5c0129410.1021/acs.energyfuels.5c01294
Xiangyang Ji, Yuhui Xia, Guilin Liu, Baiting Long, Hongyin Chen, Jian Liu and Weiyu Song*,
{"title":"CO2-Assisted Propane Dehydrogenation over Lithium-Promoted PtZn4@S-1: Unraveling the Active Sites","authors":"Xiangyang Ji, Yuhui Xia, Guilin Liu, Baiting Long, Hongyin Chen, Jian Liu and Weiyu Song*, ","doi":"10.1021/acs.energyfuels.5c0129410.1021/acs.energyfuels.5c01294","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01294https://doi.org/10.1021/acs.energyfuels.5c01294","url":null,"abstract":"<p >Constructing a bifunctional active site to boost propane dehydrogenation (PDH) in tandem with the reverse water gas reaction (RWGS) showed great potential in meeting the supply of olefins, while the crucial role of the bifunctional active sites is still unclear. Herein, a combination of kinetic and spectroscopic evidence was utilized to confirm the nonuniform bifunctional site distribution of the PtZn<sub>4</sub>@S-1 catalyst. Then, lithium atoms were incorporated to tune the bifunctional sites. A series of characterizations indicated that the introduction of lithium suppressed the incorporation of Zn atoms into the framework of silicalite-1 zeolite. As a result, the nanosized Pt<sub><i>x</i></sub>Zn<sub><i>y</i></sub> clusters were converted into larger Li<sub><i>z</i></sub>Pt<sub><i>x</i></sub>Zn<sub><i>y</i></sub> clusters with a higher Pt–Pt coordination number. This led to decreased PDH activity and stability, which confirmed that the real active sites of PDH are nanosized Pt<sub><i>x</i></sub>Zn<sub><i>y</i></sub> clusters anchored by the framework Zn atoms. However, the lithium atoms showed a volcano curve with CO<sub>2</sub> conversion. When the atomic mole ratio of Li to Pt was 34, it showed the highest CO<sub>2</sub> conversion, indicating that the Si-OLi species and the Li<sub><i>z</i></sub>Pt<sub><i>x</i></sub>Zn<sub><i>y</i></sub> clusters were directly involved in the CO<sub>2</sub> activation process. Further treatment of the Li<sub>34</sub>PtZn<sub>4</sub>@S-1 catalysts with water washing converted the Si-OLi species back to Si–OH species. This change had little influence on the PDH activity, while the RWGS showed nearly no activity, confirming that the real active site of CO<sub>2</sub> activation is the synergy between the Li<sub><i>z</i></sub>Pt<sub><i>x</i></sub>Zn<sub><i>y</i></sub> clusters and Si-OLi species.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10572–10580 10572–10580"},"PeriodicalIF":5.2,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211774","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Energy & FuelsPub Date : 2025-05-21DOI: 10.1021/acs.energyfuels.5c0050810.1021/acs.energyfuels.5c00508
Mudassar Maraj, Amima Butt, Sarmad Ali*, Ali Haider, Faisal Ali, Naeem Abas Kalair, Nian Li*, Zhenyang Wang and Xiuhong Li*,
{"title":"Bifunctional TeS/TeP2O7 Nanocomposite for Enhanced Energy Storage and Hydrogen Evolution","authors":"Mudassar Maraj, Amima Butt, Sarmad Ali*, Ali Haider, Faisal Ali, Naeem Abas Kalair, Nian Li*, Zhenyang Wang and Xiuhong Li*, ","doi":"10.1021/acs.energyfuels.5c0050810.1021/acs.energyfuels.5c00508","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00508https://doi.org/10.1021/acs.energyfuels.5c00508","url":null,"abstract":"<p >Finding cost-effective and efficient nanomaterials to address the energy crisis is a significant challenge for energy production and storage technologies. Herein, tellurium-based sulfide (TeS) and phosphate (TeP<sub>2</sub>O<sub>7</sub>) as well as their nanocomposite (TeS/TeP<sub>2</sub>O<sub>7</sub>) are prepared via a solvothermal process. The structure of these TeS and TeP<sub>2</sub>O<sub>7</sub> based nanomaterials are characterized by XRD, SEM, EDX, TEM, and HRTEM, while their electrochemical analysis involves cyclic voltammetry, electrochemical impedance spectroscopy, and linear sweep voltammetry. The synthesized materials exhibit a large surface area and porous structure, forming spherical nanoflowers with petal thicknesses of about 20–25 nm, which enables boosting the electrochemical performance. The prepared electrode of the TeS/TeP<sub>2</sub>O<sub>7</sub> active material shows redox behavior and a noticeable improvement in specific capacitance (<i>C</i><sub>s</sub>) of 1552.2 Fg<sup>–1</sup> at 1 Ag<sup>–1</sup> calculated from galvanostatic charge–discharge (GCD) measurements. These nanocomposites also show excellent cyclic stability with capacity retention of 91.5% after 5000 GCD cycles. In addition to its energy-storage capabilities, the TeS/TeP<sub>2</sub>O<sub>7</sub> nanocomposite exhibits exceptionally improved electrocatalytic performance with lower HER overpotential (281 mV) and Tafel slope (44 mVdec<sup>–1</sup>) and also higher H<sub>2</sub> production rate (197 μmolh<sup>–1</sup>g<sup>–1</sup>). The spherical nanoflowers of TeS/TeP<sub>2</sub>O<sub>7</sub> highlight the material’s potential for dual applications in supercapacitor electrodes as well as efficient catalysts for hydrogen production.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10659–10673 10659–10673"},"PeriodicalIF":5.2,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}